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[Display omitted] • The simulation results successfully guided the preparation of the insulating paper. • Nano-SiO 2 enhances the interfacial binding and compatibility of composite fiber. • Nano-SiO 2 improved the mechanical and insulating properties of the insulating paper. • Nano-SiO 2 reduced the energy barrier of composite fiber and reduce polarization loss. Following the surge in power loads and continuous improvement in the voltage level, insulating papers' mechanical and electrical properties face new challenges. However, traditional inefficient "tentative" trial and error experiments are formidable to rapidly and efficiently prepare cellulose composite insulating paper because the direct scientific theory or simulation guidance is insufficient. To solve this problem, the nano-silica(nano-SiO 2)/polyimide(PI)/cellulose composite models were designed and their mechanical, and dielectric properties were predicted by molecular dynamics (MD) simulation. The preparation of corresponding nano-SiO 2 /PI/cellulose insulating paper was guided by the MD simulation results and their surface morphology, mechanical properties, and electrical properties were investigated. The experimental results are in good agreement with the MD simulation results and confirmed that P3 insulating paper possesses the best comprehensive performance, and its tensile strength, relative permittivity, dielectric loss, volume resistivity, and breakdown strength are 71.44 MPa, 2.39, 0.2%, 5.16 × 1015 Ω∙m, and 75.8 kV∙mm−1, respectively. This work proves the feasibility and effectiveness of using MD simulation to guide the development of new insulating papers, and compared with the existing traditional preparation methods, this method is expected to be applied to study various new materials in the future and promote the vigorous development of new materials. [ABSTRACT FROM AUTHOR]